Recent work on controlling the three-dimensional morphology of nano- and micro-sized objects has included an increasing number of studies on scrolls. The scroll form is attractive because it is a structure with open ends and edges, adjustable interlayer distances, and flexible interior volume that can be used for cargo transport. Some nanostructured heterolayer systems are known to exhibit scrolling behavior, and the major efforts have involved metal and metal oxide (especially semiconductor) multilayers deposited on a sacrificial material layer. Upon etching (removing the sacrificial layer), the released heterostructures spontaneously roll into micrometer-sized scrolls/tubes. However, new materials and new techniques to fabricate such functional nano- and microsized scrolls need to be explored to extend the application and lower the cost.